Anomalous Interfacial Electron-Transfer Kinetics in Twisted Trilayer Graphene Caused by Layer-Specific Localization

Kaidi Zhang; Yun Yu; Stephen Carr; Mohammad Babar; Ziyan Zhu; Bryan Junsuh Kim; Catherine Groschner; Nikta Khaloo; Takashi Taniguchi; Kenji Watanabe; Venkatasubramanian Viswanathan; D. Kwabena Bediako

doi:10.1021/acscentsci.3c00326

論文 Anomalous Interfacial Electron-Transfer Kinetics in Twisted Trilayer Graphene Caused by Layer-Specific Localization

Kaidi Zhang ; Yun Yu ; Stephen Carr ; Mohammad Babar ; Ziyan Zhu ; Bryan Junsuh Kim ; Catherine Groschner ; Nikta Khaloo ; Takashi Taniguchi (National Institute for Materials Science) ; Kenji Watanabe (National Institute for Materials Science) ; Venkatasubramanian Viswanathan ; D. Kwabena Bediako

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Kaidi Zhang, Yun Yu, Stephen Carr, Mohammad Babar, Ziyan Zhu, Bryan Junsuh Kim, Catherine Groschner, Nikta Khaloo, Takashi Taniguchi, Kenji Watanabe, Venkatasubramanian Viswanathan, D. Kwabena Bediako. Anomalous Interfacial Electron-Transfer Kinetics in Twisted Trilayer Graphene Caused by Layer-Specific Localization. ACS Central Science. 2023, 9 (6), 1119-1128. https://doi.org/10.1021/acscentsci.3c00326

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(abstract)

Interfacial electron-transfer (ET) reactions underpin the interconversion of electrical and chem- ical energy. Pioneering experiments showed that the ET rate depends on the Fermi–Dirac dis- tribution of the electronic density of states (DOS) of the electrode, formalized in the Marcus– Hush–Chidsey (MHC) model. Here, by controlling interlayer twists in well-defined trilayer graphene moir ́es, we show that ET rates are strikingly dependent on electronic localization in each atomic layer, and not the overall DOS. The large degree of tunability inherent to moir ́e electrodes leads to local ET kinetics that range over three orders of magnitude across different constructions of only three atomic layers, even exceeding rates at bulk metals. Our results demonstrate that beyond the ensemble DOS, electronic localization is critical in facilitating interfacial ET, with implications for understanding the origin of high interfacial reactivity typ- ically exhibited by defects at electrode–electrolyte interfaces.

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